(33b) DNA Origami Self-Assembly into Superstructures Via Explicit Characterization and Optimization of the Thermodynamics and Kinetics of the Assembly Process

The hierarchical self-assembly of different types of DNA origami
nanostructure components into well-defined complexes would make it
possible to build larger DNA nanostructures where locations across the
structure (up to a micron in scale) can be addressed with nanometer
scale precision. These structures could serve as templates for novel
biomolecular devices for sensing cellular interactions for the design
of metamaterials.

However, such self-assembly processes have typically been plagued by
low yields that drop rapidly as complex size increases. To understand
more about how DNA origami structures self-assemble into complexes, we
constructed origami monomers designed to self-assemble into
heterotetrameric ring structures via specific Watson-Crick base
pairing interactions. We used fluorescence spectroscopy to
characterize how origami interface structure and design control the
kinetics and thermodynamics of dimerization, and correlation
fluorescence microscopy to characterize the thermodynamics of all of
the reactions in the assembly. We used this information to optimize
the assembly process of both origami complexes with well-formed
structure and the assembly of 2-dimensional origami lattices.